Polyolefins,
such as polyethylene and polypropylene, are globally
the most widely used plastics and are considered to be essential materials.
Because they lack polar groups, polyolefins are poorly adhesive, which
poses serious recycling challenges. Here, we describe a novel adhesion
system involving a polyurethane adhesive and an untreated polyolefin,
in which the interface is tightly bound by needle-like polyolefin
crystals in the same way that nails adhere to wood. The polyurethane
and polyolefin inter-diffuse at high temperatures to form a mixed
interfacial layer, after which the polyolefin recrystallizes in the
layer upon cooling. Polyurethanes with optimally balanced non-polar
and polar blocks exhibit superior adhesion due to their larger miscibility
windows, polyolefin compatibilities, and the resulting long needle-like
polyolefin crystals.